Blood‐Capillary‐Inspired,Free‐Standing,Flexible, and Low‐Cost Super‐Hydrophobic N‐CNTs@SS Cathodes for High‐Capacity,High‐Rate,and Stable Li‐Air Batteries

With the rising demand for flexible and wearable electronic devices, flexible power sources with high energy densities are required to provide a sustainable energy supply. Theoretically, rechargeable, flexible Li‐O₂/air batteries can provide extremely high specific energy densities; however, the high costs, complex synthetic methods, and inferior mechanical properties of the available flexible cathodes severely limit their practical applications. Herein, inspired by the structure of human blood capillary tissue, this study demonstrates for the first time the in situ growth of interpenetrative hierarchical N‐doped carbon nanotubes on the surface of stainless‐steel mesh (N‐CNTs@SS) for the fabrication of a self‐supporting, flexible electrode with excellent physicochemical properties via a facile and scalable one‐step strategy. Benefitting from the synergistic effects of the high electronic conductivity and stable 3D interconnected conductive network structure, the Li‐O₂ batteries obtained with the N‐CNTs@SS cathode exhibit superior electrochemical performance, including a high specific capacity (9299 mA h g^?1 at 500 mA g^?1), an excellent rate capability, and an exceptional cycle stability (up to 232 cycles). Furthermore, as‐fabricated flexible Li‐air batteries containing the as‐prepared flexible super‐hydrophobic cathode show excellent mechanical properties, stable electrochemical performance, and superior H₂O resistibility, which enhance their potential to power flexible and wearable electronic devices.     

Resolution of 1‐n‐Butyl‐3‐Methyl‐3‐Phospholene 1‐Oxide With TADDOL Derivatives and Calcium Salts of O,O'‐Dibenzoyl‐(2R,3R)‐ or O,O'‐di‐p‐Toluoyl‐(2R,3R)‐tartaric Acid

The resolution methods applying (?)‐(4R,5R)‐4,5‐bis(diphenylhydroxymethyl)‐2,2‐dimethyldioxolane (“TADDOL”), (?)‐(2R,3R)‐α,α,α',α'‐tetraphenyl‐1,4‐dioxaspiro[4.5]decan‐2,3‐dimethanol (“spiro‐TADDOL”), as well as the acidic and neutral Ca²⁺ salts of (?)‐O,O'‐dibenzoyl‐ and (?)‐O,O'‐di‐p‐toluoyl‐(2R,3R)‐tartaric acid were extended for the preparation of 1‐n‐butyl‐3‐methyl‐3‐phospholene 1‐oxide in optically active form. In one case, the intermediate diastereomeric complex could be identified by single‐crystal X‐ray analysis. The absolute P‐configuration of the enantiomers of the phospholene oxide was also determined by comparing the experimentally obtained and calculated CD spectra. Chirality 26:174–182, 2014. © 2014 Wiley Periodicals, Inc.     

The evaluation of acute toxicity,antimicrobial activity of 1‐phenyl‐5‐p‐tolyl‐1H‐1, 2, 3‐triazole,and binding to human serum albumin

1‐Phenyl‐5‐p‐tolyl‐1H‐1, 2, 3‐triazole (PPTA) was a synthesized compound. The result of acute toxicities to mice of PPTA by intragastric administration indicated that PPTA did not produce any significant acute toxic effect on Kunming strain mice. It exhibited the various potent inhibitory activities against two kinds of bananas pathogenic bacteria, black sigatoka and freckle, when compared with that of control drugs and the inhibitory rates were up to 64.14% and 43.46%, respectively, with the same concentration of 7.06 mM. The interaction of PPTA with human serum albumin (HSA) was studied using fluorescence polarization, absorption spectra, 3D fluorescence, and synchronous spectra in combination with quantum chemistry and molecular modeling. Multiple modes of interaction between PPTA and HSA were suggested to stabilize the PPTA–HSA complex, based on thermodynamic data and molecular modeling. Binding of PPTA to HSA induced perturbation in the microenvironment around HSA as well as secondary structural changes in the protein.     

“Water‐in‐Salt” Electrolyte Makes Aqueous Sodium‐Ion Battery Safe,Green, and Long‐Lasting

Narrow electrochemical stability window (1.23 V) of aqueous electrolytes is always considered the key obstacle preventing aqueous sodium‐ion chemistry of practical energy density and cycle life. The sodium‐ion water‐in‐salt electrolyte (NaWiSE) eliminates this barrier by offering a 2.5 V window through suppressing hydrogen evolution on anode with the formation of a Na⁺‐conducting solid‐electrolyte interphase (SEI) and reducing the overall electrochemical activity of water on cathode. A full aqueous Na‐ion battery constructed on Na_0.66[Mn_0.66Ti_0.34]O₂ as cathode and NaTi₂(PO₄)₃ as anode exhibits superior performance at both low and high rates, as exemplified by extraordinarily high Coulombic efficiency (>99.2%) at a low rate (0.2 C) for >350 cycles, and excellent cycling stability with negligible capacity losses (0.006% per cycle) at a high rate (1 C) for >1200 cycles. Molecular modeling reveals some key differences between Li‐ion and Na‐ion WiSE, and identifies a more pronounced ion aggregation with frequent contacts between the sodium cation and fluorine of anion in the latter as one main factor responsible for the formation of a dense SEI at lower salt concentration than its Li cousin.     

Claisen–Schmidt condensation: Synthesis of (1S,6R)/(1R,6S)‐2‐oxo‐N,4,6‐triarylcyclohex‐3‐enecarboxamide derivatives with different substituents in H2O/EtOH

A simple, green, and direct three‐component condensation of acetophenone, aromatic aldehydes with 3‐oxo‐N‐phenylbutanamide (acetoacetanilide) to generate some novel (1S,6R)/(1R,6S)‐2‐oxo‐N,4,6‐triarylcyclohex‐3‐enecarboxamide derivatives was carried out over K₂CO₃ (10 mol%) with high efficiency in water/ethanol as green solvent at room temperature. This protocol proceeded via Claisen–Schmidt condensation and Michael addition. The present methodology offers several advantages, such as short reaction time, high yield, more readily available and inexpensive materials, more environmentally friendly, no need for column chromatography, simple work‐up procedure, and the absence of volatile and hazardous organic solvents.     

Low‐Cost N,N′‐Bicarbazole‐Based Dopant‐Free Hole‐Transporting Materials for Large‐Area Perovskite Solar Cells

Despite the recent unprecedented development of efficient dopant‐free hole transporting materials (HTMs) for high‐performance perovskite solar cells (PSCs) on small‐area devices (≤0.1 cm²), low‐cost dopant‐free HTMs for large‐area PSCs (≥1 cm²) with high power conversion efficiencies (PCEs) have rarely been reported. Herein, two novel HTMs, 3,3′,6,6′ (or 2,2′,7,7′)‐tetrakis(N,N′‐di‐p‐methoxyphenylamine)‐N,N′‐bicarbazole (3,6 BCz‐OMeTAD or 2,7 BCz‐OMeTAD), are synthesized via an extremely simple route from very cheap raw materials. Owing to their excellent film‐forming abilities and matching energy levels, 3,6 BCz‐OMeTAD and 2,7 BCz‐OMeTAD can be successfully employed as a perfect ultrathin (≈30 nm) hole transporting layer in large‐area PSCs up to 1 cm². The 3,6 BCz‐OMeTAD and 2,7 BCz‐OMeTAD based large‐area PSCs show highest PCEs up to 17.0% and 17.6%, respectively. More importantly, high performance large‐area PSCs based on 2,7 BCz‐OMeTAD retain 90% of the initial efficiency after 2000 h storage in an ambient environment without encapsulation.     

DPP‐IV‐resistant,long‐acting oxyntomodulin derivatives

Obesity is one of the major risk factors for type 2 diabetes, and the development of agents, that can simultaneously achieve glucose control and weight loss, is being actively pursued. Therapies based on peptide mimetics of the gut hormone glucagon‐like peptide 1 (GLP‐1) are rapidly gaining favor, due to their ability to increase insulin secretion in a strictly glucose‐dependent manner, with little or no risk of hypoglycemia, and to their additional benefit of causing a modest, but durable weight loss. Oxyntomodulin (OXM), a 37‐amino acid peptide hormone of the glucagon (GCG) family with dual agonistic activity on both the GLP‐1 (GLP1R) and the GCG (GCGR) receptors, has been shown to reduce food intake and body weight in humans, with a lower incidence of treatment‐associated nausea than GLP‐1 mimetics. As for other peptide hormones, its clinical application is limited by the short circulatory half‐life, a major component of which is cleavage by the enzyme dipeptidyl peptidase IV (DPP‐IV). SAR studies on OXM, described herein, led to the identification of molecules resistant to DPP‐IV degradation, with increased potency as compared to the natural hormone. Analogs derivatized with a cholesterol moiety display increased duration of action in vivo. Moreover, we identified a single substitution which can change the OXM pharmacological profile from a dual GLP1R/GCGR agonist to a selective GLP1R agonist. The latter finding enabled studies, described in detail in a separate study (Pocai A, Carrington PE, Adams JR, Wright M, Eiermann G, Zhu L, Du X, Petrov A, Lassman ME, Jiang G, Liu F, Miller C, Tota LM, Zhou G, Zhang X, Sountis MM, Santoprete A, Capitò E, Chicchi GG, Thornberry N, Bianchi E, Pessi A, Marsh DJ, SinhaRoy R. Glucagon‐like peptide 1/glucagon receptor dual agonism reverses obesity in mice. Diabetes 2009; 58: 2258–2266), which highlight the potential of GLP1R/GCGR dual agonists as a potentially superior class of therapeutics over the pure GLP1R agonists currently in clinical use. Copyright © 2011 European Peptide Society and John Wiley & Sons, Ltd.     

SREBP‐1c,Pdx‐1, and GLP‐1R involved in palmitate–EPA regulated glucose‐stimulated insulin secretion in INS‐1 cells

Impairment of glucose‐stimulated insulin secretion (GSIS) caused by glucolipotoxicity is an essential feature in type 2 diabetes mellitus (T2DM). Palmitate and eicosapentaenoate (EPA), because of their lipotoxicity and protection effect, were found to impair or restore the GSIS in beta cells. Furthermore, palmitate was found to up‐regulate the expression level of sterol regulatory element‐binding protein (SREBP)‐1c and down‐regulate the levels of pancreatic and duodenal homeobox (Pdx)‐1 and glucagon‐like peptide (GLP)‐1 receptor (GLP‐1R) in INS‐1 cells. To investigate the underlying mechanism, the lentiviral system was used to knock‐down or over‐express SREBP‐1c and Pdx‐1, respectively. It was found that palmitate failed to suppress the expression of Pdx‐1 and GLP‐1R in SREBP‐1c‐deficient INS‐1 cells. Moreover, down‐regulation of Pdx‐1 could cause the low expression of GLP‐1R with/without palmitate treatment. Additionally, either SREBP‐1c down‐regulation or Pdx‐1 over‐expression could partially alleviate palmitate‐induced GSIS impairment. These results suggested that sequent SREBP‐1c‐Pdx‐1‐GLP‐1R signal pathway was involved in the palmitate‐caused GSIS impairment in beta cells. J. Cell. Biochem. 111: 634–642, 2010. © 2010 Wiley‐Liss, Inc.     

Comparative Effect of Quercetin and Quercetin‐3‐O‐β‐d‐Glucoside on Fibrin Polymers,Blood Clots,and in Rodent Models

The present study evaluates the in vitro, in vivo, and ex vivo antithrombotic and anticoagulant effect of two flavonoids: quercetin and quercetin‐3‐O‐β‐d ‐glucoside (isoquercetin). The present results have shown that quercetin and isoquercetin inhibit the enzymatic activity of thrombin and FXa and suppress fibrin clot formation and blood clotting. The prolongation effect of quercetin and isoquercetin against epinephrine and collagen‐induced platelet activation may have been caused by intervention in intracellular signaling pathways including coagulation cascade and aggregation response on platelets and blood. The in vivo and ex vivo anticoagulant efficacy of quercetin and isoquercetin was evaluated in thrombin‐induced acute thromboembolism model and in ICR mice. Our findings showed that in vitro and in vivo inhibitory effects of quercetin were slightly higher than that of quercetin glucoside, whereas in vitro and ex vivo anticoagulant effects of quercetin were weaker than that of quercetin glucoside because of their structural characteristics.     

Large‐scale synthesis of tert‐butyl (3R,5S)‐6‐chloro‐3,5‐dihydroxyhexanoate by a stereoselective carbonyl reductase with high substrate concentration and product yield

To biosynthesize the (3R,5S)‐CDHH in an industrial scale, a newly synthesized stereoselective short chain carbonyl reductase (SCR) was successfully cloned and expressed in Escherichia coli. The fermentation of recombinant E. coli harboring SCR was carried out in 500 L and 5000 L fermenters, with biomass and specific activity of 9.7 g DCW/L, 15749.95 U/g DCW, and 10.97 g DCW/L, 19210.12 U/g DCW, respectively. The recombinant SCR was successfully applied for efficient production of (3R,5S)‐CDHH. The scale‐up synthesis of (3R,5S)‐CDHH was performed in 5000 L bioreactor with 400 g/L of (S)‐CHOH at 30°C, resulting in a space‐time yield of 13.7 mM/h/g DCW, which was the highest ever reported. After isolation and purification, the yield and d.e. of (3R,5S)‐CDHH reached 97.5% and 99.5%, respectively. © 2017 American Institute of Chemical Engineers Biotechnol. Prog., 33:612–620, 2017     

High‐Abundance and Low‐Cost Metal‐Based Cathode Materials for Sodium‐Ion Batteries: Problems,Progress, and Key Technologies

Recently, room‐temperature stationary sodium‐ion batteries (SIBs) have received extensive investigations for large‐scale energy storage systems (EESs) and smart grids due to the huge natural abundance and low cost of sodium. The SIBs share a similar “rocking‐chair” sodium storage mechanism with lithium‐ion batteries; thus, selecting appropriate electrodes with a low cost, satisfactory electrochemical performance, and high reliability is the key point for the development for SIBs. On the other hand, the carefully chosen elements in the electrodes also largely determine the cost of SIBs. Therefore, earth‐abundant‐metal‐based compounds are ideal candidates for reducing the cost of electrodes. Among all the high‐abundance and low‐cost metal elements, cathodes containing iron and/or manganese are the most representative ones that have attracted numerous studies up till now. Herein, recent advances on both iron‐ and manganese‐based cathodes of various types, such as polyanionic, layered oxide, MXene, and spinel, are highlighted. The structure–function property for the iron‐ and manganese‐based compounds is summarized and analyzed in detail. With the participation of iron and manganese in sodium‐based cathode materials, real applications of room‐temperature SIBs in large‐scale EESs will be greatly promoted and accelerated in the near future.